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Reaction of [NiCl 2 ( PnH ) 4 ] ( 1 ) ( PnH =6‐ tert ‐butyl‐pyridazine‐3‐thione) with NiCl 2  affords the binuclear paddlewheel (PW) complex [Ni 2 ( Pn ) 4 ] ( 2 ). Diamagnetic complex  2  is the first example of a PW complex capable of reversibly binding and releasing NH 3 . The NH 3  ligand in [Ni 2 ( Pn ) 4 (NH 3 )] ( 2 ⋅NH 3 ) enforces major spectroscopic and magnetic susceptibility changes, thus displaying vapochromic properties ( λ  max ( 2 )=532 nm,  λ  max ( 2 ⋅NH 3 )=518 nm) and magnetochemical switching ( 2 :  S =0;  2 ⋅NH 3 :  S =1). Upon repeated adsorption/desorption cycles of NH 3  the PW core remains intact. Compound  2  can be embedded into thin polyurethane films ( 2  P ) under retention of its sensing abilities. Therefore,  2  qualifies as reversible optical probe for ammonia. The magnetochemical switching of  2  and  2 ⋅NH 3  was studied in detail by SQUID measurements showing that in  2 ⋅NH 3 , solely the Ni atom coordinated the NH 3  molecule is responsible for the paramagnetic behavior.

Vapochromism and Magnetochemical Switching of a Nickel(II) Paddlewheel Complex by Reversible NH 3 Uptake and Release